1110
ISSN 0030-400X, Optics and Spectroscopy, 2019, Vol. 127, No. 6, pp. 1110–1116. © Pleiades Publishing, Ltd., 2019.
Stability of Optical Responses from Lead-free Perovskite Films
E. V. Ushakova
a, b,
*, A. I. Matuhina
a
, A. V. Sokolova
a
, S. A. Cherevkov
a
, K. V. Bogdanov
a
,
A. Dubavik
a
, M. A. Baranov
a
, A. P. Litvin
a
, K. Takai
c
, A. V. Fedorov
a
, and A. V. Baranov
a
a
ITMO University, St. Petersburg, 197101 Russia
b
City University of Hong Kong, Hong Kong SAR
c
Hosei University, Tokio, 1848584 Japan
*e-mail: elena.ushakova@itmo.ru
Received April 24, 2019; revised April 24, 2019; accepted September 9, 2019
Abstract—Materials with perovskite-type crystal structure attract much attention due to their unique optical
properties, such as high quantum yield of photoluminescence and high carrier mobility. However, their fur-
ther utilization as an active media in photonic and optoelectronic devices is limited by the lack of stability of
their optical responses together with the presence of lead cations in the chemical composition. Here, a
detailed study of the optical properties and their stability under ambient conditions of perovskite films with
the chemical composition (CH
3
NH
3
)
x
A
y
I
z
, where A = Pb, Bi, Sb, was performed. The changes in optical
responses of the samples were monitored for 3 months. It was shown that the stability of perovskite films was
improved by surface passivation with a thin layer of polymethylmethacrylate onto their surface. The devel-
oped procedures of film formation and following surface passivation are of interest in the design of active opti-
cal materials based on perovskite films with the increased optical performance.
Keywords: Raman spectra, photoluminescence, bismuth, antimony, PMMA
DOI: 10.1134/S0030400X19120270
INTRODUCTION
The design and development of novel optical mate-
rials are one of the main directions of modern Material
Science. The synthesis and investigation of the optical
properties of materials with a perovskite-type crystal
structure are of both fundamental and applied scien-
tific interest. These materials attract increasing atten-
tion due to such unique properties as high carrier
mobility (caused by a high diffusion length of ~1 μm
[1]), high exciton binding energy (~50–60 meV,
allowing exciton transitions to be observed even at
room temperature [2, 3]), a high photoluminescence
(PL) quantum yield [4–8]. In particular, materials
with perovskite symmetry are in demand for solar
energy applications. To date, perovskite-based solar
cells have already achieved a conversion efficiency of
23.3% [9]. They are also in demand as an active
medium for laser radiation sources. Due to their min-
iature size and the ability to tune the emission wave-
length by modifying their chemical composition
which allows them to cover the entire visible spectrum,
they have great potential for integration into optoelec-
tronic systems [10–17].
Despite the obvious perspective of these materials,
there are a number of problems that need to be tackled
before these technologies are commercialized. One of
these problems is the presence of toxic lead cations in
the perovskite chemical composition. A possible solu-
tion is to use elements from the 14th group of the peri-
odic table instead of lead atoms, for example, tin (Sn)
and germanium (Ge) [18]. However, rapid atmo-
spheric degradation of such perovskite material upon
exposure to oxygen and water vapor, i.e. the oxidation
of Sn
2+
cations to Sn
4+
, does not allow achieving the
high stability performance under ambient [19–26].
Perovskite materials based on Ge cations have a simi-
lar tendency to oxidize to Ge
2+
[27, 28]. Other divalent
cations, for example, Sr and Ba, are also used as a sub-
stituting element for lead cation [29, 30]; however,
these materials have a large band gap which signifi-
cantly limits their applications. The perovskite-type
structure is also typical of ferroelectromagnets such as
BiFeO
3
, BiFe
2
CrO
6
, and BiMnO
3
[31–35] which
makes it possible to consider elements of the
15th group, such as bismuth (Bi) and antimony (Sb),
as a potential replacement for Pb atoms.
Taking into account the abovementioned issues,
the development of protocols for the formation of
lead-free perovskites and the study of their optical
properties are the priority tasks for the development of
this field of photovoltaics. Here, we investigated the
optical responses of lead-free perovskite thin films in
comparison with lead-based perovskite films in detail.
The efficient passivation of the film surface can be
achieved by the using of the thin polymer layer depo-
OPTICS OF LOW-DIMENSIONAL STRUCTURES,
MESOSTRUCTURES, AND METAMATERIALS